Joshua W. Kevek

Grains and grain boundaries in single-layer graphene atomic patchwork quilts

The properties of polycrystalline materials are often dominated by the size of their grains and by the atomic structure of their grain boundaries. These effects should be especially pronounced in two-dimensional materials, where even a line defect can divide and disrupt a crystal. These issues take on practical significance in graphene, which is a hexagonal, two-dimensional crystal of carbon atoms. Single-atom-thick graphene sheets can now be produced by chemical vapour deposition on scales of up to metres, making their polycrystallinity almost unavoidable. Theoretically, graphene grain boundaries are predicted to have distinct electronic, magnetic, chemical and mechanical properties that strongly depend on their atomic arrangement. Yet because of the five-order-of-magnitude size difference between grains and the atoms at grain boundaries, few experiments have fully explored the graphene grain structure. Here we use a combination of old and new transmission electron microscopy techniques to bridge these length scales. Using atomic-resolution imaging, we determine the location and identity of every atom at a grain boundary and find that different grains stitch together predominantly through pentagon–heptagon pairs. Rather than individually imaging the several billion atoms in each grain, we use diffraction-filtered imaging to rapidly map the location, orientation and shape of several hundred grains and boundaries, where only a handful have been previously reported. The resulting images reveal an unexpectedly small and intricate patchwork of grains connected by tilt boundaries. By correlating grain imaging with scanning probe and transport measurements, we show that these grain boundaries severely weaken the mechanical strength of graphene membranes but do not as drastically alter their electrical properties. These techniques open a new window for studies on the structure, properties and control of grains and grain boundaries in graphene and other two-dimensional materials.

Terahertz imaging and spectroscopy of large-area single-layer graphene.

THz imaging and spectroscopy using broadband THz pulses map out the THz carrier dynamics of a large-area graphene-on-Si sample, showing that the local sheet-conductivity varies across the sample from σ<inf>s</inf>, = 1.7×10⁻³ to 2.4×10⁻³ Ω⁻¹.

Hyperspectral Imaging of Structure and Composition in Atomically Thin Heterostructures

Precise vertical stacking and lateral stitching of two-dimensional (2D) materials, such as graphene and hexagonal boron nitride (h-BN), can be used to create ultrathin heterostructures with complex functionalities, but this diversity of behaviors also makes these new materials difficult to characterize. We report a DUV-vis-NIR hyperspectral microscope that provides imaging and spectroscopy at energies of up to 6.2 eV, allowing comprehensive, all-optical mapping of chemical composition in graphene/h-BN lateral heterojunctions and interlayer rotations in twisted bilayer graphene (tBLG). With the addition of transmission electron microscopy, we obtain quantitative structure-property relationships, confirming the formation of interfaces in graphene/h-BN lateral heterojunctions that are abrupt on a micrometer scale, and a one-to-one relationship between twist angle and interlayer optical resonances in tBLG. Furthermore, we perform similar hyperspectral imaging of samples that are supported on a nontransparent silicon/SiO2 substrate, enabling facile fabrication of atomically thin heterostructure devices with known composition and structure.

Photothermoelectric Effect in Suspended Semiconducting Carbon Nanotubes

We have performed scanning photocurrent microscopy measurements of field-effect transistors (FETs) made from individual ultraclean suspended carbon nanotubes (CNTs). We investigate the spatial-dependence, polarization-dependence, and gate-dependence of photocurrent and photovoltage in this system. While previous studies of surface-bound CNT FET devices have identified the photovoltaic effect as the primary mechanism of photocurrent generation, our measurements show that photothermoelectric phenomena play a critical role in the optoelectronic properties of suspended CNT FETs. We have quantified the photothermoelectric mechanisms and identified regimes where they overwhelm the photovoltaic mechanism.

Origins of Charge Noise in Carbon Nanotube Field-Effect Transistor Biosensors

Determining the major noise sources in nanoscale field-effect transistor (nanoFET) biosensors is critical for improving bioelectronic interfaces. We use the carbon nanotube (CNT) FET biosensor platform to examine the noise generated by substrate interactions and surface adsorbates, both of which are present in current nanoFET biosensors. The charge noise model is used as a quantitative framework to show that insulating substrates and surface adsorbates are both significant contributors to the noise floor of CNT FET biosensors. Removing substrate interactions and surface adsorbates reduces the power spectral density of background voltage fluctuations by 19-fold.

Terahertz imaging of inhomogeneous electrodynamics in single-layer graphene embedded in dielectrics

We investigate electron transport properties in large-area, single-layer graphene embedded in dielectric media, using free-space terahertz (THz) imaging and time-domain spectroscopy. Sandwiched between a thin polymethyl methacrylate (PMMA) layer and a Si substrate, graphene layers of different growth recipes exhibit distinctive spatial inhomogeneity of sheet conductivity. The non-contacting, non-destructive THz probe reveals that the PMMA layer induces a small, yet noticeable reduction in conductivity.

Single Electron Charge Sensitivity of Liquid-Gated Carbon Nanotube Transistors

Random telegraph signals corresponding to activated charge traps were observed with liquid-gated CNT FETs. The high signal-to-noise ratio that we observe demonstrates that single electron charge sensing is possible with CNT FETs in liquids at room temperature. We have characterized the gate-voltage dependence of the random telegraph signals and compared to theoretical predictions. The gate-voltage dependence clearly identifies the sign of the activated trapped charge.

Imaging Grains and Grain Boundaries in Single-Layer Graphene: An Atomic Patchwork Quilt

1. School of Applied and Engineering Physics, Cornell University, Ithaca, NY 14853, USA 2. Department of Physics, Cornell University, Ithaca, NY 14853, USA 3. Department of Chemistry and Chemical Biology, Cornell University, Ithaca, NY 14853, USA 4. Department of Physics and Astronomy, Brigham Young University, Provo, UT 84602, USA 5. Kavli Institute at Cornell for Nanoscale Science, Ithaca, NY14853, USA * These authors contributed equally to this work.

Small molecule injection into single-cell C. elegans embryos via carbon-reinforced nanopipettes.

The introduction of chemical inhibitors into living cells at specific times in development is a useful method for investigating the roles of specific proteins or cytoskeletal components in developmental processes. Some embryos, such as those of Caenorhabditis elegans, however, possess a tough eggshell that makes introducing drugs and other molecules into embryonic cells challenging. We have developed a procedure using carbon-reinforced nanopipettes (CRNPs) to deliver molecules into C. elegans embryos with high temporal control. The use of CRNPs allows for cellular manipulation to occur just subsequent to meiosis II with minimal damage to the embryo. We have used our technique to replicate classical experiments using latrunculin A to inhibit microfilaments and assess its effects on early polarity establishment. Our injections of latrunculin A confirm the necessity of microfilaments in establishing anterior-posterior polarity at this early stage, even when microtubules remain intact. Further, we find that latrunculin A treatment does not prevent association of PAR-2 or PAR-6 with the cell cortex. Our experiments demonstrate the application of carbon-reinforced nanopipettes to the study of one temporally-confined developmental event. The use of CRNPs to introduce molecules into the embryo should be applicable to investigations at later developmental stages as well as other cells with tough outer coverings.

Fabrication of low-noise carbon nanotube field-effect transistor biosensors

We report the fabrication of suspended carbon nanotube field effect transistors (CNT FETs) designed for biological sensing applications. We compare the electrical properties of our suspended CNT FET design to standard surface based CNT FETs. In particular, we show a reduction in environmental noise, suggesting that the new sensor design is a promising candidate for low-noise sensing applications.